Mechanism of layer-by-layer oxidation of Si(001) surfaces by two-dimensional oxide-island nucleation at SiO2/Si interfaces

We have studied the mechanism of layer-by-layer oxidation of Si(001) surfaces. The layer-by-layer oxidation was confirmed and precisely monitored by scanning reflection electron microscopy (SREM). By combining SREM and scanning tunneling microscopy (STM) methods, we investigated the change in atomic-scale roughness at SiO2/Si(001)interfaces during the oxidation. We found that, while the oxide interface is atomically flat after the oxidation of each layer is complete, nanometer-scale oxide islands with a single atomic height are densely nucleated at the interface during the oxidation of each layer. We also observed an oscillation in the intensity of reflection high-energy electron diffraction (RHEED) spots during the top-layer oxidation. These results clearly indicate that the layer-by-layer oxidation proceeds by the nucleation of nanometer-scale oxide islands at the interfaces and by their preferential lateral island growth.